平原河网溶解无机氮来源的稳定同位素示踪——以温瑞塘河为例

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摘要选择浙江典型平原河网—温瑞塘河为研究区,联合多种水化学参数和稳定同位素(δ¹⁵N/δ¹⁸O-NO₃^-、δ¹⁵N-NH₄⁺、δ¹⁸O-H₂O),识别了水体溶解无机氮(DIN)污染的时空分布特征和主要来源,在此基础上,构建了一种耦合硝酸盐和氨氮浓度及其同位素和贝叶斯污染源解析模型(SIAR)的DIN定量源解析方法,计算了温瑞塘河各污染源对DIN的贡献率.结果表明:温瑞塘河DIN污染严重,其浓度变化范围为1.43~12.88mg/L,氨氮、硝酸盐和亚硝酸盐分别占DIN的63%、35%和2%;DIN污染呈现明显的时空异质性,时间上DIN浓度呈现丰水期<平水期<枯水期的变化趋势,空间上呈现主河道<支流,城乡结合部河道<城市河道的特点;研究区DIN转化以硝化过程为主,反硝化过程不明显;模型计算结果显示粪便污水、土壤氮、化肥和大气沉降对丰水期水体DIN的贡献率分别为 (71.29 ± 14.24)%、(18.96 ± 13.89)%、(6.78 ± 5.91)%和 (2.97 ± 2.28)%,对平水期DIN的贡献率分别为 (57.51 ± 15.53)%、(25.01 ± 16.45)%、(15.24 ± 8.19)%和(2.25 ± 2.28)%,对枯水期DIN的贡献率分别为 (57.60 ± 16.27)%、(26.75 ± 17.58)%、(13.03 ± 7.95)%和 (2.61 ± 2.55)%;不确定性分析结果表明土壤氮和粪便污水贡献率存在较大的不确定性.本研究建立的DIN溯源方法能够有效计算不同污染源对水体DIN的贡献率,弥补了以往研究只单独解析硝酸盐或者氨氮来源的不足.

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	刘音利
	廖忠鹭
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	谭鑫敏
	王宇昊
	马浩翔
	纪晓亮

关键词 ：平原河网, 溶解无机氮, 稳定同位素, 污染源解析, SIAR模型

Abstract：In this study, a representative plain river network in Zhejiang Province, namely Wen-Rui Tang River, was selected as the research area. The spatio-temporal variations and primary pollution sources of riverine dissolved inorganic nitrogen (DIN) were identified by combining multiple hydrochemical parameter with stable isotopes (δ¹⁵N/δ¹⁸O-NO₃^-, δ¹⁵N-NH₄⁺, δ¹⁸O-H₂O). On basis of these findings, a quantitative source apportionment method of DIN was developed by integrating nitrate and ammonia concentrations, their isotope compositions, and a SIAR model. Finally, the contributions of each pollution source to riverine DIN in Wen-Rui Tang River were calculated. Results revealed that the Wen-Rui Tang River exhibited severe DIN pollution with DIN concentrations ranging from 1.43mg/L to 12.88mg/L. Ammonia, nitrate and nitrite accounted for 63%, 35%, and 2% of DIN, respectively. Significant spatio-temporal variations of DIN content were observed in the Wen-Rui Tang River. Temporally, DIN concentrations followed the order: high flow season < usual flow season < low flow season. Spatially, DIN concentrations in mainstream were lower than those in tributaries and DIN concentrations in urban-rural segments were lower than those in urban segments. The predominant transformation process of DIN was nitrification rather than denitrification within the study area. The model results revealed that the contributions of manure and sewage, soil nitrogen, nitrogen fertilizer, and atmospheric deposition to DIN during the wet season were (71.29 ± 14.24)%, (18.96 ± 13.89)%, (6.78 ± 5.91)%, and (2.97 ± 2.28)%, respectively; during the usual flow season, these contributions accounted for (57.51 ± 15.53)%, (25.01 ± 16.45)%, (15.24 ± 8.19)%, and (2.25 ± 2.28)%, respectively; during the low flow season, they constituted (57.60 ± 16.27)%, (26.75 ± 17.58)%, (13.03 ± 7.95)% and (2.61 ± 2.55)%, respectively. Stronger uncertainties associated with soil nitrogen and manure and sewage contributions were found according to the uncertainty analysis.

Key words： plain river networks dissolved inorganic nitrogen stable isotopes pollution source apportionment SIAR model

收稿日期: 2024-05-25

PACS:

X522

基金资助:国家自然科学基金资助项目(42307104);浙江省自然基金资助项目(LTGS23D030002);温州市基础性科研项目(S20220014);国家级大学生创新创业项目(202210343011);温州医科大学大学生科研课题(wyx2022101038)

通讯作者: 纪晓亮,研究员,jxl2018@iwaterlab.com E-mail: jxl2018@iwaterlab.com

作者简介: 刘音利(2001-),女,浙江宁波人,本科生,主要从事环境卫生学方面的研究.发表论文3篇.liuyinli2024@163.com.

引用本文:

刘音利, 廖忠鹭, 王芃玮, 詹晨灿, 谭鑫敏, 王宇昊, 马浩翔, 纪晓亮. 平原河网溶解无机氮来源的稳定同位素示踪——以温瑞塘河为例[J]. 中国环境科学, 2024, 44(12): 6874-6885. LIU Yin-li, LIAO Zhong-lu, WANG Peng-wei, ZHAN Chen-can, TAN Xin-min, WANG Yu-hao, MA Hao-xiang, JI Xiao-liang. Tracing dissolved inorganic nitrogen sources in plain river networks using stable isotopes: a case study of the Wen-Rui Tang River. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(12): 6874-6885.

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